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Quantifying Actinide–Carbon Bond Covalency in a Uranyl–Aryl Complex Utilizing Solution <sup>13</sup>C NMR Spectroscopy

Osvaldo Ordoñez, Xiaojuan Yu, Guang Wu, Jochen Autschbach, Trevor W. Hayton

2023Inorganic Chemistry14 citationsDOIOpen Access PDF

Abstract

Reaction of [UO 2 Cl 2 (THF) 2 ] 2 with in situ generated LiFmes (FmesH = 1,3,5-(CF 3 ) 3 C 6 H 3 ) in Et 2 O resulted in the formation of the uranyl aryl complexes [Li(THF) 3 ][UO 2 (Fmes) 3 ] ([Li(THF) 3 ][ 1 ]) and [Li(Et 2 O) 3 (THF)][UO 2 (Fmes) 3 ] ([Li(Et 2 O) 3 (THF)][ 1 ]) in good to moderate yields after crystallization from hexanes and Et 2 O, respectively. Both complexes were characterized by X-ray crystallography and NMR spectroscopy. DFT calculations reveal that the C ispo resonance in [ 1 ] − exhibits a deshielding of 51 ppm from spin–orbit coupling effects originating at uranium, which indicates an appreciable covalency in the U–C bonding interaction.

Topics & Concepts

ChemistryUranylArylActinideNuclear magnetic resonance spectroscopyUraniumCrystallizationCrystallographySpectroscopyInorganic chemistryPhysical chemistryStereochemistryOrganic chemistryIonMetallurgyMaterials scienceQuantum mechanicsAlkylPhysicsRadioactive element chemistry and processingNuclear Materials and PropertiesRadioactive contamination and transfer